张静静, 凌丽霞, 马彩萍, 章日光, 王宝俊. RhnNin合金团簇尺寸对RhnNin/TiO2催化合成气制乙醇性能的影响[J]. 燃料化学学报(中英文). DOI: 10.1016/S1872-5813(24)60454-8
引用本文: 张静静, 凌丽霞, 马彩萍, 章日光, 王宝俊. RhnNin合金团簇尺寸对RhnNin/TiO2催化合成气制乙醇性能的影响[J]. 燃料化学学报(中英文). DOI: 10.1016/S1872-5813(24)60454-8
ZHANG Jingjing, LING Lixia, MA Caiping, ZHANG Riguang, WANG Baojun. Effect of the RhnNin/TiO2 alloy cluster size on the catalytic performance of RhnNin/TiO2 in the conversion of syngas to ethanol[J]. Journal of Fuel Chemistry and Technology. DOI: 10.1016/S1872-5813(24)60454-8
Citation: ZHANG Jingjing, LING Lixia, MA Caiping, ZHANG Riguang, WANG Baojun. Effect of the RhnNin/TiO2 alloy cluster size on the catalytic performance of RhnNin/TiO2 in the conversion of syngas to ethanol[J]. Journal of Fuel Chemistry and Technology. DOI: 10.1016/S1872-5813(24)60454-8

RhnNin合金团簇尺寸对RhnNin/TiO2催化合成气制乙醇性能的影响

Effect of the RhnNin/TiO2 alloy cluster size on the catalytic performance of RhnNin/TiO2 in the conversion of syngas to ethanol

  • 摘要: 本工作采用密度泛函理论(DFT)和微观动力学方法研究了不同Rh-Ni合金团簇尺寸的RhnNin/TiO2(n = 1、2、3、4)催化剂上的合成气制乙醇反应。结果表明,Rh1Ni1/TiO2和Rh3Ni3/TiO2能够显著促进CO活化转化及C−C链的形成,并抑制甲烷的生成。其中,Rh1Ni1/TiO2表现出最高的乙醇生成活性和相对选择性。电子性质分析表明,在Rh1Ni1/TiO2催化剂上,合金团簇上Ni原子及载体上Ti和O原子向Rh原子转移的电荷最多,合金团簇上Rh-Ni间相互作用最强,且合金团簇与TiO2载体间的相互作用也最强,其催化活性最高。在525 K下,从头算分子动力学模拟(AIMD)模拟显示Rh1Ni1/TiO2催化剂具有较高的热稳定性。

     

    Abstract: The direct conversion of syngas to ethanol on the RhnNin/TiO2 (n = 1, 2, 3, 4) catalyst has been investigated by using the density functional theory (DFT) and micro-kinetic methods, in order to elucidate the regulatory mechanism of RhnNin alloy cluster size-induced metal-support interaction on the catalytic performance of RhnNin/TiO2 in the ethanol synthesis. The results indicate that Rh1Ni1/TiO2 and Rh3Ni3/TiO2 can significantly enhance the conversion of CO and the formation of C−C bond and meanwhile inhibit the generation of methane. Rh1Ni1/TiO2 exhibits the highest ethanol production activity and relative selectivity. The electronic property analysis results suggest that Ni atoms on the alloy clusters and Ti and O atoms on the supports transfer the most charge to the Rh atoms on the Rh1Ni1/TiO2 catalyst, which displays the strongest Rh-Ni interaction on the alloy clusters as well as the strongest interaction between the alloy clusters and the TiO2 support, endowing Rh1Ni1/TiO2 with the highest catalytic activity. In addition, the Ab-initio molecular dynamics (AIMD) simulations at 525 K show that the Rh1Ni1/TiO2 catalyst has high thermal stability.

     

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